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The appearance of very low emittance, high-power synchrotron sources has resulted in ever longer beamlines, often requiring a very weak curvature on the mirrors that transport the beam to the experiment, where the radius of curvature is on the order of kilometers. Manufacturing weakly curved, low figure error grazing incidence mirrors is difficult as the mirrors must be manufactured to an accuracy comparable to the wavelength of the transmitted light. Often the delivered mirrors have figure errors at various length scales (general shape, slope errors, roughness), which compromise image quality. An error in general shape, like the radii of a toroidal mirror, results in long-sighted or short-sighted imaging that is not so simply corrected by changing the distances and incidence angles as the mirror controls the beam focus in both vertical and horizontal directions; for a toroidal mirror, the tangential and sagittal radii need to match correctly for the desired focusing effect. Adaptive downstream optics can compensate for this. In this paper, an alternative method to reduce the sensitivity to a large radius error outside the specified tolerance range in the first mirror of a plane grating monochromator beamline at MAX IV is presented. It is found that distributed focusing by two passive, fixed radius mirrors reduces greatly the sensitivity to the radius errors in both mirrors. The radius tolerance of a mirror initially found to be unacceptable for single stage focusing is easily accommodated on both mirrors in distributed focusing, without compromising the imaging capability.
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FinEstBeAMS (Finnish-Estonian Beamline for Atmospheric and Materials Sciences) is a multidisciplinary beamline constructed at the 1.5â GeV storage ring of the MAX IV synchrotron facility in Lund, Sweden. The beamline covers an extremely wide photon energy range, 4.5-1300â eV, by utilizing a single elliptically polarizing undulator as a radiation source and a single grazing-incidence plane grating monochromator to disperse the radiation. At photon energies below 70â eV the beamline operation relies on the use of optical and thin-film filters to remove higher-order components from the monochromated radiation. This paper discusses the performance of the beamline, examining such characteristics as the quality of the gratings, photon energy calibration, photon energy resolution, available photon flux, polarization quality and focal spot size.
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The SPECIES beamline has been transferred to the new 1.5â GeV storage ring at the MAXâ IV Laboratory. Several improvements have been made to the beamline and its endstations during the transfer. Together the Ambient Pressure X-ray Photoelectron Spectroscopy and Resonant Inelastic X-ray Scattering endstations are capable of conducting photoelectron spectroscopy in elevated pressure regimes with enhanced time-resolution and flux and X-ray scattering experiments with improved resolution and flux. Both endstations offer a unique capability for experiments at low photon energies in the vacuum ultraviolet and soft X-ray range. In this paper, the upgrades on the endstations and current performance of the beamline are reported.
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HIPPIE is a soft X-ray beamline on the 3â GeV electron storage ring of the MAXâ IV Laboratory, equipped with a novel ambient-pressure X-ray photoelectron spectroscopy (APXPS) instrument. The endstation is dedicated to performing in situ and operando X-ray photoelectron spectroscopy experiments in the presence of a controlled gaseous atmosphere at pressures up to 30â mbar [1â mbar = 100â Pa] as well as under ultra-high-vacuum conditions. The photon energy range is 250 to 2200â eV in planar polarization and with photon fluxes >1012â photonsâ s-1 (500â mA ring current) at a resolving power of greater than 10000 and up to a maximum of 32000. The endstation currently provides two sample environments: a catalysis cell and an electrochemical/liquid cell. The former allows APXPS measurements of solid samples in the presence of a gaseous atmosphere (with a mixture of up to eight gases and a vapour of a liquid) and simultaneous analysis of the inlet/outlet gas composition by online mass spectrometry. The latter is a more versatile setup primarily designed for APXPS at the solid-liquid (dip-and-pull setup) or liquid-gas (liquid microjet) interfaces under full electrochemical control, and it can also be used as an open port for ad hoc-designed non-standard APXPS experiments with different sample environments. The catalysis cell can be further equipped with an IR reflection-absorption spectrometer, allowing for simultaneous APXPS and IR spectroscopy of the samples. The endstation is set up to easily accommodate further sample environments.
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In this paper, we examine decay and fragmentation of core-excited and core-ionized water molecules combining quantum chemical calculations and electron-energy-resolved electron-ion coincidence spectroscopy. The experimental technique allows us to connect electronic decay from core-excited states, electronic transitions between ionic states, and dissociation of the molecular ion. To this end, we calculate the minimum energy dissociation path of the core-excited molecule and the potential energy surfaces of the molecular ion. Our measurements highlight the role of ultra-fast nuclear motion in the 1a1 -14a1 core-excited molecule in the production of fragment ions. OH+ fragments dominate for spectator Auger decay. Complete atomization after sequential fragmentation is also evident through detection of slow H+ fragments. Additional measurements of the non-resonant Auger decay of the core-ionized molecule (1a1 -1) to the lower-energy dication states show that the formation of the OH+ + H+ ion pair dominates, whereas sequential fragmentation OH+ + H+ â O + H+ + H+ is observed for transitions to higher dication states, supporting previous theoretical investigations.
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We have studied the dissociation of the trifluoromethane molecule, CHF3 , into negative ionic fragments at the C 1s and F 1s edges. The measurements were performed by detecting coincidences between negative and positive ions. We observed five different negative ions: F- , H- , C- , CF- , and F2 - . Their production was confirmed by the analysis of triple coincidence events (negative-ion/positive-ion/positive-ion or NIPIPI coincidences) that were recorded with cleaner signals than those of the negative-ion/positive-ion coincidences. The intensities of the most intense NIPIPI coincidence channels were recorded as a function of photon energy across the C 1s and F 1s excitations and ionization thresholds. We also observed dissociation channels involving the formation of one negative ion and three positive ions. Our results demonstrate that negative-ion/positive-ion coincidence spectroscopy is a very sensitive method to observe anions, which at inner-shell edges are up to three orders of magnitude less probable dissociation products than cations.
Assuntos
Ânions/análise , Clorofluorcarbonetos de Metano/química , Cátions/análise , Elétrons , Espectrometria de Massas/métodosRESUMO
We have studied the fragmentation of the methanol molecule after core excitation and core ionization by observing coincidences between negative and positive ions. Five different negative ions (H-, C-, CH-, O-, and OH-) were observed at both the C 1s and O 1s edges. As negative ion formation occurs after resonant and normal Auger decay of core-hole states, it is necessarily linked with the release of positively charged fragments. Our data show that such fragmentation can happen in many different ways: We found approximately 30 negative-ion/positive-ion/positive-ion coincidence (NIPIPICO) channels. All involve only singly charged positive ions. Fragmentation channels leading to atomic ions are the most probable, but positive molecular ions are also frequently found in the context of anion formation. Coincidence yields as a function of photon energy were determined for the most intense NIPIPICO channels. Adding together the data measured at different photon energies, we could also verify the occurrence of four-ion coincidences, which involved one negative ion (H- or O-) and three positive ions.
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SPECIES is an undulator-based soft X-ray beamline that replaced the old I511 beamline at the MAX II storage ring. SPECIES is aimed at high-resolution ambient-pressure X-ray photoelectron spectroscopy (APXPS), near-edge X-ray absorption fine-structure (NEXAFS), X-ray emission spectroscopy (XES) and resonant inelastic X-ray scattering (RIXS) experiments. The beamline has two branches that use a common elliptically polarizing undulator and monochromator. The beam is switched between the two branches by changing the focusing optics after the monochromator. Both branches have separate exit slits, refocusing optics and dedicated permanent endstations. This allows very fast switching between two types of experiments and offers a unique combination of the surface-sensitive XPS and bulk-sensitive RIXS techniques both in UHV and at elevated ambient-pressure conditions on a single beamline. Another unique property of the beamline is that it reaches energies down to approximately 27â eV, which is not obtainable on other current APXPS beamlines. This allows, for instance, valence band studies under ambient-pressure conditions. In this article the main properties and performance of the beamline are presented, together with selected showcase experiments performed on the new setup.
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We report yields of mass-resolved negative ions and positive ions measured in coincidence after core excitation of water molecules. The analysis of negative-ion/positive-ion and negative-ion/positive-ion/positive-ion coincidence events provides new information on pathways leading to negative ion production, enhancing the present understanding of the dissociation processes of the water molecule. Dissociation following (resonant) Auger decay dominates negative ion production, but radiative decay is shown to contribute above the O 1s ionization threshold. A peak in the H(-)/O(+) yield above the O 1s threshold is attributed to decay from doubly excited states.
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A high precision five rotation-axes polarimeter using transmission multilayers as polarizers and reflection multilayers as analyzers has been designed and manufactured. To cover the extreme ultraviolet regime, Mo/Si, Cr/C, Sc/Cr, and W/B4C multilayers for transmission and reflection have also been designed and produced. The polarimeter mechanics is supported on a hexapod to simplify the alignment relative to photon beam. The instrument is designed so that it can be easily transferred between different beamlines.
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We present a newly constructed spectrometer for negative-ion/positive-ion coincidence spectroscopy of gaseous samples. The instrument consists of two time-of-flight ion spectrometers and a magnetic momentum filter for deflection of electrons. The instrument can measure double and triple coincidences between mass-resolved negative and positive ions with high detection efficiency. First results include identification of several negative-ion/positive-ion coincidence channels following inner-shell photoexcitation of sulfur hexafluoride (SF6).
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The distinct optical emission from ZnO materials, nanoneedles and microcrystallites synthesized with different sizes and morphologies by a flow deposition technique, is investigated with X-ray excited optical luminescence (XEOL) and time-resolved X-ray excited optical luminescence (TR-XEOL) from a synchrotron light source at the O K and Zn L(3,2) edges. The innovative use of XEOL, allowing site-specific chemical information and luminescence information at the same time, is fundamental to provide direct evidence for the different behaviour and the crucial role of bulk and surface defects in the origin of ZnO optical emission, including dynamics. XEOL from highly crystalline ZnO nanoneedles is characterized by a sharp band-gap emission (~380 nm) and a broad red luminescence (~680 nm) related to surface defects. Luminescence from ZnO microcrystallites is mostly dominated by green emission (~510 nm) associated with defects in the core. TR-XEOL experiments show considerably faster decay dynamics in nanoneedles compared to microcrystallites for both band-gap emission and visible luminescence. Herein we make a fundamental step forward correlating for the first time the interplay of size, crystallinity, morphology and excitation energy with luminescence from ZnO materials.
Assuntos
Nanoestruturas/química , Óxido de Zinco/química , Luminescência , Medições Luminescentes , Nanoestruturas/ultraestrutura , Raios XRESUMO
The carbon 1s photoelectron spectrum of CF4 measured at photon energies from 330 to 1500 eV shows significant contributions from nonsymmetric vibrational modes. These increase linearly as the photon energy increases. The excitation of these modes, which is not predicted in the usual Franck-Condon point of view, arises from the recoil momentum imparted to the carbon atom in the ionization process. A theory is presented for quantitative prediction of the recoil effect; the predictions of this theory are in agreement to the measurements. The experiments also yield the vibrational frequencies of the symmetric and asymmetric stretching modes in core-ionized CF4, the change in CF bond length upon ionization, -0.61 pm, and the Lorentzian linewidth of the carbon 1s hole, 67 meV.
RESUMO
The boron 1s photoelectron spectrum of (11)BF(3) has been measured at a photon energy of 400 eV and a resolution of about 55 meV. The pronounced vibrational structure seen in the spectrum has been analyzed to give the harmonic and anharmonic vibrational frequencies of the symmetric stretching mode, 128.1 and 0.15 meV, as well as the change in equilibrium BF bond length upon ionization, -5.83 pm. A similar change in bond length has been observed for PF(3) and SiF(4), but a much smaller change for CF(4). Theoretical calculations for BF(3) that include the effects of electron correlation give results that are in reasonable accord with the experimental values. The Lorentzian (lifetime) width of the boron 1s core hole in BF(3) is found to be 72 meV, comparable to the value of 77 meV that has been reported for CF(4).